The micro Raman spectra of solid-liquid boundary layer, the melts and crystal side, were measured at real time, concerning BSO crystal grown with zone-melting method. The structure characters in boundary layer, melts and crystal were analyzed. The process, of which the growth unit structure changed while they transited from melts through boundary layer to crystal lattice, was analyzed. The results show that, there exists Bi3O4 and [SiO4] bonding structure in the melts of BSO crystal. While in the solid-liquid boundary layer, the Bi3O4 molecular units converge into [BiO7] octahedron monomer of polymer in form, the monomer or the polymer converge with the [SiO4] structure units, then all these converged structure enter into crystal lattice sites.
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